Thanks to its ultrahigh carrier mobility (∼104-105 cm2 V-1 s-1), graphene shows tremendous application potential in nanoelectronics, but it cannot be applied in effective field-effect transistors (FETs) because of its intrinsic gapless band structure. Thus, introducing a bandgap for graphene is a prerequisite to realize an FET for logic applications. Herein, through first-principles GW calculations, we have predicted a series of novel Dion-Jacobson (DJ) phase halide perovskite semiconductors CsSb(Br1-xIx)4 (x = 0, 0.5, 1) with the quasi-linear (graphene-like) band edge dispersion; as the best one of which, CsSbBr2I2 exhibits a direct bandgap (0.52 eV) as well as a quasi-linear electronic dispersion, yielding an ultrasmall carrier effective mass (0.03 m0) and a high estimated carrier mobility (5 × 103 cm2 V-1 s-1). This gives a significant reference to the exploration of semiconductors with excellent transport properties. Moreover, our calculations also implicate that the DJ perovskites CsSb(Br1-xIx)4 (x = 0, 0.25, 0.5, 0.75, 1) show soft and anisotropic mechanical characteristics as well as excellent electronic, transport, and optical properties, which demonstrate their multifunctional application in infrared optoelectronic, high-speed electronics, and photovoltaics.
Keywords: Dion−Jacobson phase perovskite; Sb-based perovskite; first-principles calculation; quasi-linear band edge dispersion; spin−orbit coupling effect; strong optical absorption.